洞庭湖血吸虫病疫区表层水中酚类分布特征及健康风险研究
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摘要
本研究选取湖南省典型血吸虫病疫区为研究对象,以三峡库区为对照研究区,针对洞庭湖血吸虫病疫区的81个表层水样和三峡库区的47个表层水样中的多种酚类化合物的污染特征和潜在风险进行分析。同时,建立和优化了酚类化合物的高灵敏串联质谱定量分析方法,并对酚类化合物衍生化条件进行优化,确立了五氟苄基溴(PFBBr)衍生化,GC/MS联用测定水样中多种酚类化合物的分析检测方法。对两研究区共128个表层水样依次进行SPE萃取,五氟苄基溴衍生化,GC/MS定性定量分析,并采用SPSS进行统计分析,结合酚类化合物迁移降解规律和环境化学、水文、地质、气候等学科知识,全面探讨污染物在研究区表层水中的分布特征和潜在风险,以期为该地区地表水中酚类化合物污染现状的评估提供参考依据。主要研究结果如下；
(1)建立并优化了五氟苄基溴衍生化、GC/MS联用测定表层水中多种酚类化合物的方法。确定了水浴温度为30℃,水浴时间25min,碳酸钾添加量0.2g时为最佳衍生化条件,本方法检出限(≤218.18pg·L-1)满足了低于1gg·L-1浓度级超痕量分析的要求。通过对7个高浓度和7个低浓度样品进行加标回收率重复性试验,得到低浓度时回收率为72%-123.7%,相对标准偏差为8.0%-27.6%。高浓度时回收率为72.3%-119%,相对标准偏差为7%-12.8%。此测定方法实验结果表明改进后的五氟苄基溴衍生化,GC/MS联用同时测定水样中多种酚类化合物的方法简便易行、试剂材料易获得、试验条件易控制,且回收率和试验重复性可接受,满足了同时检出环境水样中存在多种酚类组分的要求。
(2)首次研究了我国最典型湖沼型疫区(洞庭湖区)及三峡库区的酚类化合物污染,并对表层水样中同时存在的多种酚类组分进行了系统研究。结果显示洞庭湖典型血吸虫病疫区中的沱江、藕池河下游、松澧洪道这3条河流平水期水样中酚类含量最高,总浓度为：1362.64-2436.53ng·L-1,同一河流不同水期表层水样中的∑酚类浓度存在显著性差异(P<0.05,T检验),同一水期不同河流之间∑酚类浓度差别不大(P>0.05,T检验),处于同一污染水平。苯酚、2.6-二氯酚、2-硝基酚、五氯酚在三个不同水期中被检出浓度均较高,浓度分别为ND-1783.89ng·L-1、0.01-362.72ng·L-1、0.02-11908.22ng·L-1、ND-6057.37ng·L-1,分别占总酚类的13.8%、1%、54.7%、26.9%,是该研究区在三个不同水期检出的主要酚类化合物。三峡库区干流和支流表层水样中酚类总浓度的几何均值分别为52.47和87.99ng·L-1。干流和支流中非氯酚类总浓度的几何均值均大于氯酚类,库区表层水以非氯代酚组分为主。苯酚、邻甲酚和2-硝基酚是库区干流水样中主要的酚类,分别占干流∑酚类的79.1%、3.7%和3.6%。苯酚、邻甲酚、2,6-二氯酚和2-硝基酚是库区支流水样中的优势污染物,分别占支流∑酚类的77.5%、5.4%、3.8%和2.2%。
(3)分析了洞庭湖研究区酚类污染潜在风险。洞庭湖研究区表层水样中检出的苯酚、2.6-二氯酚、2-硝基酚、五氯酚浓度低于《国家污染物环境健康风险名录》、GB3838-2002和GB5749-2006中的标准限值,对当地水环境安全带来的潜在风险较小。研究结果中三个不同水期PCP(五氯酚)的检出浓度与文献报导的国内其他血吸虫病疫区水样中的浓度相比,显示该研究区水样中PCP的浓度处于各疫区的中等污染水平,五氯酚及其降解产物的污染会给当地水环境带来潜在风险。三峡库区表层水中检出的苯酚和2-硝基酚的检出浓度与《国家污染物环境健康风险名录》中的标准限值相比较,远低于可能导致生物毒性危害的标准限值,与国内外其他地区水体中苯酚含量相比也处于较低污染水平,三峡库区表层水样中苯酚与2-硝基酚污染给研究区水环境带来的潜在风险较小。
This study selected the typical Schistosome-endemic Areas as the research object, and taking the Three Gorges Reservoir as the contrast area. in order to investigate the pollution characteristics of a variety of phenolic compounds from81surface water samples collected from Dongting lake research area. and the47surface water samples collected from the Three Gorges Reservoir were also investigated. the high sensitive tandem mass spectrometry (ms) quantitative analysis method of the phenolic compounds was established and optimized.the control conditions of derivatization reaction were optimized.and the phenolic compounds were simultaneous determined by using PFBBr derivatization and GC-MS.this analysis and determination method was established in this study.the128surface water samples were dealed by SPE extraction. PFBBr derivatization, qualitative and quantitative analysis by GC-MS, and the data was dealed by SPSS17.0. combining with phenolic compounds migration-degradation rule and environmental chemical, hydrology, geology, and climate knowledge. and roundly discussing the distribution characteristics and potential risks of the pollutants from the research area.so as to provide important reference for evaluating the pollution situation of phenolic compounds in surface water from the local area. the main research results are as follows:
(1) Establishing and optimizing the method of analysis and determination, the best derivative condition was ascertained, the water bath temperature is30℃, the water bath time is25min, potash adding amount is0.2g. the LOD (≤218.18pg/L) of this method is much lower than lμg/L, through the recovery repeatability tests of the seven high concentration and seven low concentration samples, the test results in the low level of concentration show that the recovery is72%~123.7%, the relative standard deviation is8.0%~27.6%.and the recovery is72.3%~119%, the relative standard deviation is7%~12.8%in the low level of concentration, the experimental results show that the improved the method of analysis and determination is easier to implement, reagents and material are easy to access, test conditions are also easy to control, the recovery and test repeatability is acceptable.it contents the detection requirements of a variety of phenolic constituent from Nature water.
(2) The first study of phenolic compounds pollution from the most typical lake-swamp type epidemic areas and three gorges reservoir area have been done. donging the system research on the variety of phenolic compounds existed simultaneously in surface water samples. the results from Dongting lake research area show that the highest total concentrations of the14phenolic compounds in the three rivers were from the medium water period. the total concentration are1362.64-2436.53ng·L-1(geometric mean), there is significant difference between the concentrations of phenols in these samples from one river in different period (P <0.05,T test). there is no significant difference between the concentrations of phenols in different rivers in same period (P>0.05,T test, and the pollution level is in the same order of magnitude. the concentration of Phenol,2,6-Dichlorophenol,2-Nitrophenol and PCP detected from these three rivers in different periods are the highest, the concentrations are separately ND～1783.89ng·L-1、0.01～362.72ng·L-1、0.02～11908.22ng·L-1、ND～6057.37ng·L-1, which respectively accounted for13.8%、1%、54.7%%、26.9%in total content of phenols, they are the most predominant phenolic compounds. The results from the Three Gorges Reservoir show that the concentrations of phenolic compounds in the samples from the main stream and tributaries were52.47ng·L-1and87.99ng·L-1, respectively. The concentrations of non-chlorinated phenols were higher than those of chlorinated phenols in the main stream and tributaries, and so the non-chlorinated phenols were the predominant compounds in these surface water samples. Phenol, o-cresol and2-nitrophenol were the predominant compounds accounted for79.1%,3.7%,and3.6%in the samples from the main stream, respectively. Phenol, o-cresol,2,6-dichlorophenol and2-nitrophenol were the main compounds accounted for77.5%,5.4%,3.8%and2.2%in the samples from the tributaries, respectively.
(3) Analyzing the potential risks of phenolic pollution from the Dong Ting lake research area. as compared the concentrations of phenol2,6-Dichlorophenol2-Nitrophenol and PCP with the standard limits in National Environmental Health Risk List, GB3838-2002and GB5749-2006, the levels of these compounds were much lower than the standard limits, suggesting negligible risk of these four predominant phenolic compounds in these samples. Comparing the concentration of PCP in different period with the results reported in the other schistosome-endemic areas, the levels of PCP reported in this study were in the moderate levels order of magnitude in these schistosome-endemic areas, the pollution of PCP, and it's derivatives will lead to the potential risk of local water environment, comparing the concentrations of phenol and2-nitrophenol from the Three Gorges Reservoir research area with the standard limits in The National Environmental Health Risk List, the levels of phenol and2-nitrophenol were much lower than the standard limits, suggesting negligible risk of phenol and2-nitrophenol in these samples.
(1)建立并优化了五氟苄基溴衍生化、GC/MS联用测定表层水中多种酚类化合物的方法。确定了水浴温度为30℃,水浴时间25min,碳酸钾添加量0.2g时为最佳衍生化条件,本方法检出限(≤218.18pg·L-1)满足了低于1gg·L-1浓度级超痕量分析的要求。通过对7个高浓度和7个低浓度样品进行加标回收率重复性试验,得到低浓度时回收率为72%-123.7%,相对标准偏差为8.0%-27.6%。高浓度时回收率为72.3%-119%,相对标准偏差为7%-12.8%。此测定方法实验结果表明改进后的五氟苄基溴衍生化,GC/MS联用同时测定水样中多种酚类化合物的方法简便易行、试剂材料易获得、试验条件易控制,且回收率和试验重复性可接受,满足了同时检出环境水样中存在多种酚类组分的要求。
(2)首次研究了我国最典型湖沼型疫区(洞庭湖区)及三峡库区的酚类化合物污染,并对表层水样中同时存在的多种酚类组分进行了系统研究。结果显示洞庭湖典型血吸虫病疫区中的沱江、藕池河下游、松澧洪道这3条河流平水期水样中酚类含量最高,总浓度为：1362.64-2436.53ng·L-1,同一河流不同水期表层水样中的∑酚类浓度存在显著性差异(P<0.05,T检验),同一水期不同河流之间∑酚类浓度差别不大(P>0.05,T检验),处于同一污染水平。苯酚、2.6-二氯酚、2-硝基酚、五氯酚在三个不同水期中被检出浓度均较高,浓度分别为ND-1783.89ng·L-1、0.01-362.72ng·L-1、0.02-11908.22ng·L-1、ND-6057.37ng·L-1,分别占总酚类的13.8%、1%、54.7%、26.9%,是该研究区在三个不同水期检出的主要酚类化合物。三峡库区干流和支流表层水样中酚类总浓度的几何均值分别为52.47和87.99ng·L-1。干流和支流中非氯酚类总浓度的几何均值均大于氯酚类,库区表层水以非氯代酚组分为主。苯酚、邻甲酚和2-硝基酚是库区干流水样中主要的酚类,分别占干流∑酚类的79.1%、3.7%和3.6%。苯酚、邻甲酚、2,6-二氯酚和2-硝基酚是库区支流水样中的优势污染物,分别占支流∑酚类的77.5%、5.4%、3.8%和2.2%。
(3)分析了洞庭湖研究区酚类污染潜在风险。洞庭湖研究区表层水样中检出的苯酚、2.6-二氯酚、2-硝基酚、五氯酚浓度低于《国家污染物环境健康风险名录》、GB3838-2002和GB5749-2006中的标准限值,对当地水环境安全带来的潜在风险较小。研究结果中三个不同水期PCP(五氯酚)的检出浓度与文献报导的国内其他血吸虫病疫区水样中的浓度相比,显示该研究区水样中PCP的浓度处于各疫区的中等污染水平,五氯酚及其降解产物的污染会给当地水环境带来潜在风险。三峡库区表层水中检出的苯酚和2-硝基酚的检出浓度与《国家污染物环境健康风险名录》中的标准限值相比较,远低于可能导致生物毒性危害的标准限值,与国内外其他地区水体中苯酚含量相比也处于较低污染水平,三峡库区表层水样中苯酚与2-硝基酚污染给研究区水环境带来的潜在风险较小。
This study selected the typical Schistosome-endemic Areas as the research object, and taking the Three Gorges Reservoir as the contrast area. in order to investigate the pollution characteristics of a variety of phenolic compounds from81surface water samples collected from Dongting lake research area. and the47surface water samples collected from the Three Gorges Reservoir were also investigated. the high sensitive tandem mass spectrometry (ms) quantitative analysis method of the phenolic compounds was established and optimized.the control conditions of derivatization reaction were optimized.and the phenolic compounds were simultaneous determined by using PFBBr derivatization and GC-MS.this analysis and determination method was established in this study.the128surface water samples were dealed by SPE extraction. PFBBr derivatization, qualitative and quantitative analysis by GC-MS, and the data was dealed by SPSS17.0. combining with phenolic compounds migration-degradation rule and environmental chemical, hydrology, geology, and climate knowledge. and roundly discussing the distribution characteristics and potential risks of the pollutants from the research area.so as to provide important reference for evaluating the pollution situation of phenolic compounds in surface water from the local area. the main research results are as follows:
(1) Establishing and optimizing the method of analysis and determination, the best derivative condition was ascertained, the water bath temperature is30℃, the water bath time is25min, potash adding amount is0.2g. the LOD (≤218.18pg/L) of this method is much lower than lμg/L, through the recovery repeatability tests of the seven high concentration and seven low concentration samples, the test results in the low level of concentration show that the recovery is72%~123.7%, the relative standard deviation is8.0%~27.6%.and the recovery is72.3%~119%, the relative standard deviation is7%~12.8%in the low level of concentration, the experimental results show that the improved the method of analysis and determination is easier to implement, reagents and material are easy to access, test conditions are also easy to control, the recovery and test repeatability is acceptable.it contents the detection requirements of a variety of phenolic constituent from Nature water.
(2) The first study of phenolic compounds pollution from the most typical lake-swamp type epidemic areas and three gorges reservoir area have been done. donging the system research on the variety of phenolic compounds existed simultaneously in surface water samples. the results from Dongting lake research area show that the highest total concentrations of the14phenolic compounds in the three rivers were from the medium water period. the total concentration are1362.64-2436.53ng·L-1(geometric mean), there is significant difference between the concentrations of phenols in these samples from one river in different period (P <0.05,T test). there is no significant difference between the concentrations of phenols in different rivers in same period (P>0.05,T test, and the pollution level is in the same order of magnitude. the concentration of Phenol,2,6-Dichlorophenol,2-Nitrophenol and PCP detected from these three rivers in different periods are the highest, the concentrations are separately ND～1783.89ng·L-1、0.01～362.72ng·L-1、0.02～11908.22ng·L-1、ND～6057.37ng·L-1, which respectively accounted for13.8%、1%、54.7%%、26.9%in total content of phenols, they are the most predominant phenolic compounds. The results from the Three Gorges Reservoir show that the concentrations of phenolic compounds in the samples from the main stream and tributaries were52.47ng·L-1and87.99ng·L-1, respectively. The concentrations of non-chlorinated phenols were higher than those of chlorinated phenols in the main stream and tributaries, and so the non-chlorinated phenols were the predominant compounds in these surface water samples. Phenol, o-cresol and2-nitrophenol were the predominant compounds accounted for79.1%,3.7%,and3.6%in the samples from the main stream, respectively. Phenol, o-cresol,2,6-dichlorophenol and2-nitrophenol were the main compounds accounted for77.5%,5.4%,3.8%and2.2%in the samples from the tributaries, respectively.
(3) Analyzing the potential risks of phenolic pollution from the Dong Ting lake research area. as compared the concentrations of phenol2,6-Dichlorophenol2-Nitrophenol and PCP with the standard limits in National Environmental Health Risk List, GB3838-2002and GB5749-2006, the levels of these compounds were much lower than the standard limits, suggesting negligible risk of these four predominant phenolic compounds in these samples. Comparing the concentration of PCP in different period with the results reported in the other schistosome-endemic areas, the levels of PCP reported in this study were in the moderate levels order of magnitude in these schistosome-endemic areas, the pollution of PCP, and it's derivatives will lead to the potential risk of local water environment, comparing the concentrations of phenol and2-nitrophenol from the Three Gorges Reservoir research area with the standard limits in The National Environmental Health Risk List, the levels of phenol and2-nitrophenol were much lower than the standard limits, suggesting negligible risk of phenol and2-nitrophenol in these samples.
引文
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